Picosecond laser ultrasonic techniques for acoustic wave generation and detection have been employed to probe shear acoustic waves in liquid glycerol at gigahertz frequencies. The experimental approach uses a unique laser pulse shaping technique and a crystallographically canted metal layer to generate frequency-tunable transverse acoustic waves, and uses time-domain coherent Brillouin scattering to detect the waves after they propagate through a liquid layer and into a solid substrate. A linear frequency dependence is found for both the shear speed and attenuation rate in glycerol. DOI: 10.1103/PhysRevLett.102.107402 PACS numbers: 78.20.Hp, 43.35.+d, 78.40.Dw, 78.47.JÀ Fast structural relaxation dynamics in liquids continue to pose major fundamental challenges [1], in large measure because direct experimental access to key relaxing degrees of freedom over the time or frequency ranges of interest remains elusive. Both density and shear relaxation play central roles in the complex structural responses of viscoelastic materials. On slow time scales, dynamic mechanical analysis and sonic or related measurement methods can be used, while faster responses require measurements of longitudinal and shear acoustic waves in the megahertz and gigahertz frequency ranges. Much of the MHz range is now accessible to ultrasonics and impulsive stimulated thermal or Brillouin scattering (impulsive stimulated thermal or Brillouin scattering [2-5]), and (usually isolated) frequencies in the low GHz range may be accessed through spontaneous Brillouin scattering [6]. Recent work in x-ray Brillouin scattering has accessed THz longitudinal acoustic frequency ranges [7], but frequencies in the tens to hundreds of GHz range, where fast relaxation features occur, have remained difficult to access. Deep-UV Brillouin scattering from longitudinal acoustic waves in this range has been demonstrated [4,7], but its utility is limited by strong absorption in most materials. Picosecond ultrasonics [8], in which a short optical pulse generates a single-cycle acoustic pulse that is observed after propagation through a sample, has provided tabletop access to much of the GHz-frequency range for longitudinal acoustic waves. Adaptations of the method to enable GHz shear wave generation [9][10][11][12] have been developed. However, shear waves in liquids have remained elusive, to the extent that the challenges in ''seeking shear waves in liquids with picoseconds ultrasonics'' [13] have been elaborated explicitly. The use of multiple optical pulses to generate frequency-tunable, multiple-cycle longitudinal waves [14] has been demonstrated to improve acoustic spectral brightness for characterization of frequency-dependent material responses. Here we demonstrate this approach for generation of frequency-tunable shear as well as longitudinal acoustic waves in the GHz-frequency range. We further demonstrate a sample and optical configuration that permit the measurements to be conducted in viscoelastic liquids, whose GHz-frequency acoustic responses are of...